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The structural, electronic and magnetic behavior of the as-cast and annealed Mn₅₂Al₄₆Ti₂ and Mn₅₀Al₄₆Ti₄ alloys have been studied through electronic band structure calculations, X-ray diffraction and magnetic measurements in the temperature range 4–850 K and magnetic field up to 7 T. Band structure calculations show a preference for Ti atoms to occupy the Mn sites in the plane of Al atoms with their magnetic moments (−0.68 μ_B/Ti) coupled antiparallel relative to the Mn magnetic moments in the plane of Mn atoms (2.33 μ_B/Mn). The as-cast and annealed samples were phase mixtures with different values of the hard ferromagnetic τ phase content. Except the as-cast and annealed at 1050 °C Mn₅₂Al₄₆Ti₂ alloys, all the analyzed samples include, along with the τ and γ₂ phases, a soft κ phase (CsCl - structure type) with T_C around 530 K. The best magnetic characteristics were obtained for Mn₅₂Al₄₆Ti₂ alloy …